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Title: Protection of inorganic semiconductors for sustained, efficient photoelectrochemical water oxidation

Abstract

Small-band-gap (E g < 2 eV) semiconductors must be stabilized for use in integrated devices that convert solar energy into the bonding energy of a reduced fuel, specifically H 2 (g) or a reduced-carbon species such as CH 3 OH or CH 4 . To sustainably and scalably complete the fuel cycle, electrons must be liberated through the oxidation of water to O 2 (g). Strongly acidic or strongly alkaline electrolytes are needed to enable efficient and intrinsically safe operation of a full solar-driven water-splitting system. But, under water-oxidation conditions, the small-band-gap semiconductors required for efficient cell operation are unstable, either dissolving or forming insulating surface oxides. Here, we describe herein recent progress in the protection of semiconductor photoanodes under such operational conditions. We specifically describe the properties of two protective overlayers, TiO 2 /Ni and NiO x , both of which have demonstrated the ability to protect otherwise unstable semiconductors for > 100 h of continuous solar-driven water oxidation when in contact with a highly alkaline aqueous electrolyte (1.0 M KOH(aq)). Furthermore, the stabilization of various semiconductor photoanodes is reviewed in the context of the electronic characteristics and a mechanistic analysis of the TiO 2 films, along with amore » discussion of the optical, catalytic, and electronic nature of NiO x films for stabilization of semiconductor photoanodes for water oxidation.« less

Authors:
 [1];  [1];  [2];  [3];  [1];  [1];  [3];  [4];  [5];  [3];  [4];  [6]
+ Show Author Affiliations
  1. California Inst. of Technology (CalTech), Pasadena, CA (United States). Division of Chemistry and Chemical Engineering, Joint Center for Artificial Photosynthesis
  2. California Inst. of Technology (CalTech), Pasadena, CA (United States). Division of Chemistry and Chemical Engineering, Joint Center for Artificial Photosynthesis, Beckman Inst.
  3. California Inst. of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source
  5. California Inst. of Technology (CalTech), Pasadena, CA (United States). Division of Chemistry and Chemical Engineering
  6. California Inst. of Technology (CalTech), Pasadena, CA (United States). Division of Chemistry and Chemical Engineering, Joint Center for Artificial Photosynthesis, Beckman Inst., Kavli Nanoscience Inst.
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1379158
Alternate Identifier(s):
OSTI ID: 1358892
Grant/Contract Number:  
AC02-05CH11231; SC0004993
Resource Type:
Accepted Manuscript
Journal Name:
Catalysis Today
Additional Journal Information:
Journal Volume: 262; Journal Issue: C; Journal ID: ISSN 0920-5861
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; artificial photosynthesis; photoelectrochemistry; corrosion; catalysis

Citation Formats

Lichterman, Michael F., Sun, Ke, Hu, Shu, Zhou, Xinghao, McDowell, Matthew T., Shaner, Matthew R., Richter, Matthias H., Crumlin, Ethan J., Carim, Azhar I., Saadi, Fadl H., Brunschwig, Bruce S., and Lewis, Nathan S. Protection of inorganic semiconductors for sustained, efficient photoelectrochemical water oxidation. United States: N. p., 2015. Web. doi:10.1016/j.cattod.2015.08.017.
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Lichterman, Michael F., Sun, Ke, Hu, Shu, Zhou, Xinghao, McDowell, Matthew T., Shaner, Matthew R., Richter, Matthias H., Crumlin, Ethan J., Carim, Azhar I., Saadi, Fadl H., Brunschwig, Bruce S., & Lewis, Nathan S. Protection of inorganic semiconductors for sustained, efficient photoelectrochemical water oxidation. United States. https://doi.org/10.1016/j.cattod.2015.08.017
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Lichterman, Michael F., Sun, Ke, Hu, Shu, Zhou, Xinghao, McDowell, Matthew T., Shaner, Matthew R., Richter, Matthias H., Crumlin, Ethan J., Carim, Azhar I., Saadi, Fadl H., Brunschwig, Bruce S., and Lewis, Nathan S. Sun . "Protection of inorganic semiconductors for sustained, efficient photoelectrochemical water oxidation". United States. https://doi.org/10.1016/j.cattod.2015.08.017. https://www.osti.gov/servlets/purl/1379158.
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@article{osti_1379158,
title = {Protection of inorganic semiconductors for sustained, efficient photoelectrochemical water oxidation},
author = {Lichterman, Michael F. and Sun, Ke and Hu, Shu and Zhou, Xinghao and McDowell, Matthew T. and Shaner, Matthew R. and Richter, Matthias H. and Crumlin, Ethan J. and Carim, Azhar I. and Saadi, Fadl H. and Brunschwig, Bruce S. and Lewis, Nathan S.},
abstractNote = {Small-band-gap (E g < 2 eV) semiconductors must be stabilized for use in integrated devices that convert solar energy into the bonding energy of a reduced fuel, specifically H 2 (g) or a reduced-carbon species such as CH 3 OH or CH 4 . To sustainably and scalably complete the fuel cycle, electrons must be liberated through the oxidation of water to O 2 (g). Strongly acidic or strongly alkaline electrolytes are needed to enable efficient and intrinsically safe operation of a full solar-driven water-splitting system. But, under water-oxidation conditions, the small-band-gap semiconductors required for efficient cell operation are unstable, either dissolving or forming insulating surface oxides. Here, we describe herein recent progress in the protection of semiconductor photoanodes under such operational conditions. We specifically describe the properties of two protective overlayers, TiO 2 /Ni and NiO x , both of which have demonstrated the ability to protect otherwise unstable semiconductors for > 100 h of continuous solar-driven water oxidation when in contact with a highly alkaline aqueous electrolyte (1.0 M KOH(aq)). Furthermore, the stabilization of various semiconductor photoanodes is reviewed in the context of the electronic characteristics and a mechanistic analysis of the TiO 2 films, along with a discussion of the optical, catalytic, and electronic nature of NiO x films for stabilization of semiconductor photoanodes for water oxidation.},
doi = {10.1016/j.cattod.2015.08.017},
journal = {Catalysis Today},
number = C,
volume = 262,
place = {United States},
year = {Sun Oct 25 00:00:00 EDT 2015},
month = {Sun Oct 25 00:00:00 EDT 2015}
}
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Publisher's Version of Record
https://doi.org/10.1016/j.cattod.2015.08.017
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    journal, January 2017

    • Laskowski, Forrest A. L.; Nellist, Michael R.; Venkatkarthick, Radhakrishnan
    • Energy & Environmental Science, Vol. 10, Issue 2
    • DOI: 10.1039/c6ee03505a

    Degradation and regeneration mechanisms of NiO protective layers deposited by ALD on photoanodes
    journal, January 2019

    • Ros, Carles; Andreu, Teresa; David, Jérémy
    • Journal of Materials Chemistry A, Vol. 7, Issue 38
    • DOI: 10.1039/c9ta08638b

    Monolithic Photoelectrochemical Device for 19% Direct Water Splitting
    text, January 2017

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